Equipment and Separation Units for Flow Chemistry Applications and Process Development

Process development and small‐scale production gets more and more important in fine chemistry and pharmaceutical production. An equipment toolbox assists process synthesis presented in this contribution. A microfluidic calorimeter can measure kinetic and thermodynamic reaction data with commercial plate reactors. A tubular reactor coiled with 90° bends allows for long residence time with low axial dispersion, also known as coiled flow inverter (CFI). A similar setup is used for continuous‐flow cooling crystallization. Small‐scale columns with rotating internals are employed for distillation and liquid‐liquid extraction. Main emphasis will be put on automation and scale‐up in future steps.     

Casson流体层流反应器中连串反应的产品分布

引　言目前化工流体力学涉及的范围已由传统的牛顿流体发展到非牛顿流体 .常见的非牛顿流体包括幂律流体、Bingham流体和Casson流体 .有许多高聚物反应物系和生化反应物系属于非牛顿流体 .特别是某些生化反应系统 ,所处理的物系常由各种天然物质组成 ,因而表现出典型的非牛顿流     

微型流化床反应器液相冷态进样停留时间分布模拟与实验

为了得出气、液相流量变化对微型流化床反应器液相停留时间的影响规律,借助Fluent软件对反应器内部流场进行数值模拟,得到其速度、压力分布特性和反应器出口液相浓度的变化曲线。采用示踪剂侧面脉冲进样法,实验测定了反应器中液相的停留时间分布。结果表明,气相流量和液相流量均对液相停留时间有明显的影响,气、液相流量为4¹0L/h时,液相平均停留时间可以控制在1.1110L/h时,液相平均停留时间可以控制在1.11¹.89s;气、液相流量的增加均会导致液相停留时间的减少,但气相流量对停留时间的影响要大于液相流量对液相停留时间的影响。数值模拟与实验数据对比分析发现二者结果吻合良好,模型可用。     

Residence time measurements in a coal hydrogenation process

Residence time of coal in the University of Utah “coiled tube” coal hydrogenation reactor has been measured. This has been done with an electronic device which detects a tracer (usually iron) as it passes specific places at the beginning and end of the reactor. The measured coal solids residence time in the reactor has varied from a few seconds to a few minutes. Calculated vapor and gas residence times are one or two seconds. Short vapor residence time terminates further hydrogenation of vapors and thus reduces gas production and hydrogen consumption. The relatively longer coal solids residence time permits further hydrogenation which increases liquid yields.     

Residence time distribution of the liquid in gas-liquid cocurrent upflow fixed-bed reactors

The authors present an experimental investigation of the residence time distribution (RTD) of the liquid in a gas-liquid upflow fixed-bed reactor with porous and nonporous particles and air/Newtonian or non-Newtonian systems. The piston-dispersion-exchange model with Danckwerts boundary conditions was used to describe the liquid flow. In the case of porous particles, the dynamic evolution of the tracer concentration in the particles was described in terms of diffusion phenomena. An imperfect pulse method was used to estimate the model parameters directly from the experimentally nonideal input and output response.     

循环浆态床气体停留时间分布的研究

研究了循环浆态床气流段的气流量和液体循环量对气体停留时间分布的影响。实验结果表明,减小气流量或者增加液体循环量,气体返混程度变大,气体平均停留时间增长。建立模型模拟循环浆态床气流段气体停留时间分布,得到停留时间分布密度函数和物料分率p与射流相似准数Ct和气液动量比准数Cr的关联式。从关联式看出,气液动量比准数Cr越小,物料分率p越大,表明循环液体流量越大,气体停留时间分布越接近于全混流。这一结论与实验结果相符。     

Modular Coiled Flow Inverter with Narrow Residence Time Distribution for Process Development and Production

The ideal plug flow reactor is a common model with narrow residence time distribution in reaction engineering. This contribution explains a design strategy of a coiled flow inverter (CFI) with narrow residence time and flexible adjustable process conditions. The design space diagram illustrates the design limits of inner diameter and coil diameter on the base of dimensionless numbers. Standard coil tube diameters allow for rational design of a limited number of devices. The reactor performance diagram enables the facile scale‐up and adaption of new process conditions with the CFI with economic boundary conditions.     

The residence time distribution for laminar flow in helically coiled tubes

Sizable errors exist in previously published studies on the residence time distribution for ideal laminar flow in a helically coiled tubes. The numerical methods used to give corrected results are generally useful for flow situations where the projections of the streamlines on the channel cross-section are closed curves.An asymptotic solution, valid at long residence times, has been obtained. This solution confirms the numerical observation that the tail of the distribution is similar to that for laminar flow in a straight tube. If molecular diffusion is ignored, this form of asymptotic behavior is shown to be a general characteristic of all flow systems involving a fixed wall. When diffusion is considered, the asymptotic residence time distribution will be a decaying exponential in time. This confirms the widespread experimental observation that residence time distributions have exponential tails.     

Residence time distribution and modeling of the liquid phase in an impinging stream reactor

Based on some experimental investigations of liquid phase residence time distribution (RTD) in an impinging stream reactor, a two-dimensional plug-flow dispersion model for predicting the liquid phase RTD in the reactor was proposed. The calculation results of the model can be in good agreement with the experimental RTD under different operating conditions. The axial liquid dispersion coefficient increases monotonously with the increasing liquid flux, but is almost independent of gas flux. As the liquid flux and the gas flux increase, the liquid dispersion coefficient of center-to-wall decreases. The axial liquid dispersion coefficient is much larger than that of center-to-wall, which indicates that the liquid RTD is dominated mainly by axial liquid dispersion in the impinging stream reactor.     

Residence time distribution and modeling of the liquid phase in an impinging stream reactor

Based on some experimental investigations of liquid phase residence time distribution (RTD) in an impinging stream reactor, a two-dimensional plug-flow dispersion model for predicting the liquid phase RTD in the reactor was proposed. The calculation results of the model can be in good agreement with the experimental RTD under different operating conditions. The axial liquid dispersion coefficient increases monotonously with the increasing liquid flux, but is almost independent of gas flux. As the liquid flux and the gas flux increase, the liquid dispersion coefficient of center-to-wall decreases. The axial liquid dispersion coefficient is much larger than that of center-to-wall, which indicates that the liquid RTD is dominated mainly by axial liquid dispersion in the impinging stream reactor.     

幂律流体三维脉动流场数值模拟

利用ANSYS软件，模拟了振动诱导单螺杆挤出机熔体输送段中非牛顿幂律流体的三维脉动流场，得到了三维脉动流场的瞬时速度分布及螺槽中物料的流动轨迹。结果表明，在脉动流场作用下，非牛顿流体的瞬时速度响应与在驱动壁面上所施加的正弦形式的脉动驱动形式不同，横螺槽方向的环流中心位置受幂律指数影响，且发生周期性改变。振动的引入使得在相同的时间内，物料的流动路程增加，且可增大物料的平均停留时间，有利于改善混合效果。     

基于丝网探针的螺旋管内气液两相流气泡行为研究

核反应堆蒸汽发生器的传热面由螺旋管束组成。螺旋管的三维螺旋结构使得泡状流和塞状流等气液两相流中的气泡在重力、离心力和浮力等作用下在管道内部呈现不对称的相分布状态,两相滑移速度增大,显著影响换热性能并导致DNB型传热恶化难以预测。实验介质为空气-水,结合自主开发的电导式丝网探针技术并发展先进的数据后处理算法,实现了复杂流场的三维时空重构和离散气泡粒径的精细测量,获得了螺旋管内泡状流和塞状流的截面空泡分布规律。基于研究结果,可根据气泡分布规律对螺旋管道的几何结构进行调整以避免传热恶化,为螺旋管式蒸发器的安全设计提供了基础数据和优化思路。     

基于丝网探针的螺旋管内气液两相流气泡行为研究

核反应堆蒸汽发生器的传热面由螺旋管束组成。螺旋管的三维螺旋结构使得泡状流和塞状流等气液两相流中的气泡在重力、离心力和浮力等作用下在管道内部呈现不对称的相分布状态,两相滑移速度增大,显著影响换热性能并导致DNB型传热恶化难以预测。实验介质为空气-水,结合自主开发的电导式丝网探针技术并发展先进的数据后处理算法,实现了复杂流场的三维时空重构和离散气泡粒径的精细测量,获得了螺旋管内泡状流和塞状流的截面空泡分布规律。基于研究结果,可根据气泡分布规律对螺旋管道的几何结构进行调整以避免传热恶化,为螺旋管式蒸发器的安全设计提供了基础数据和优化思路。     

RTD for diffusion-free laminar flow of non-newtonian fluids through coiled tubes

The residence time distribution (RTD) for diffusion-free laminar helical flow of non-Newtonian fluids has been numerically computed for values of the power-law index from 0.2 to 2.0. Experimental verification is also provided. Excellent agreement is also shown with independently calculated RTD's appearing in the literature.     

A flow model for non-newtonian liquids inside a slot die

A one-dimensional flow model for non-Newtonian liquids inside a dual-cavity slot die is presented. The model is capable of analyzing slot dies of any cavity shape, cavity taper, slot-length variations, and slot-gap variations. The proposed model incorporates a truncated-power-law model for the viscosity of non-Newtonian liquids. According to flow models with power-law approximation for liquid viscosity, the distribution of non-Newtonian liquid through a slot die depends on the slot Reynolds number only. With our model, we find that the zero shear viscosity and the relaxation time of a non-Newtonian liquid have large effects on its distribution. For non-Newtonian liquids which are expected to experience shear-thinning over portion of a slot die, it is concluded that a flow model with a truncated-power-law approximation for liquid viscosity be used to predict the liquid distribution from the die.     

Experimental Study on a Co-current Gas–Liquid Down Flow Contactor with Gas Entrainment by a Liquid Jet

Two-phase flow co-current vertical downflow reactor with gas entrainment by a liquid jet is investigated in an air–water system. Experiments are carried out in order to clarify the flow behavior of the reactor under various conditions. Gas entrainment flow rates and gas holdup are quantified experimentally and their dependency on the liquid jet flow rates are shown. The experimental program also included determination of liquid phase residence time distribution (RTD) characteristics for different liquid jet flow rates. The result of the analysis of the liquid phase RTD curves justified the tank-in-series model flow for the liquid phase. On the basis of these analyses, the reactor hydrodynamics are modeled by the tank-in-series model including dead zones. Good agreement is obtained between theoretical and experimental results assuming the reactor is operating as perfectly mixed. The volumetric mass transfer coefficient k_La_Lis determined experimentally by a “gasing out” method. The interfacial area is deduced from the bubble diameter measurements which are determined by visualization experiments.     

On a mathematical model for loop reactors—II. Estimation of parameters

Based on a model of loop reactors with sections of different mixing behaviour and on an approximation formula for its residence time distribution, a procedure is derived to determine the main model parameters, the mean circulation time, the circulation variance and the corresponding values of the individual sections. Finally the results of application of this procedure to RTD-measurements in a laboratory liquid jet loop reactor are presented.     

多层三相流化床流动特性的研究

针对多层三相流化床进行冷模试验,以饱和KCl溶液为示踪剂,采用电导法测定不同液速、气速和固相浓度条件下液相流体在床内的停留时间分布曲线、平均停留时间。采用多釜串联模型得到模拟参数以及其返混特性随着各操作参数变化的情况。结果表明：液相速度对平均停留时间影响显著,随液速增大而急剧减小;气速和载体对平均停留时间影响较小,随着气速和载体量增加平均停留时间均呈下降趋势。液相返混程度随气相速度增加而增加,随液相速度和载体含量的增加而减小。     

Trickle bed reactor diluted with fine particles and coiled tubular flow-type reactor for kinetic measurements without external effects

Gas and liquid velocities in laboratory scale trickle bed reactors are one or two orders of magnitude lower than those in commercial reactors. Then, the kinetic data may include the external effects. This shortcoming of laboratory scale trickle bed reactor can be resolved by diluting the catalyst bed with fine inert particles. The catalyst bed dilution increases dynamic liquid holdup, pressure drop, gas–liquid mass transfer coefficient. Hydrogenation of 2-phenylpropene on Pd/Al₂O₃ was performed with the trickle bed reactor diluted with fine inert particles and the coiled tubular flow-type reactor to compare the kinetics with that of the basket type batch reactor. The trickle bed reactor diluted with fine inert particles is suitable to obtain the reaction rate without external effects even if the liquid velocity is low. The coiled tubular flow-type reactor should be used at high gas velocities.